Mechanistic study of partial oxidation of methane to syngas using in situ time-resolved FTIR and microprobe Raman spectroscopies
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In situ time-resolved Fourier transform infrared (FTIR) and microprobe Raman spectroscopies were used to characterize the reaction mechanisms of the partial oxidation of methane to syngas over SiO2- and gamma-Al2O3-supported rhodium and ruthenium catalysts. The interaction of both pure methane and a methane/oxygen mixture at a stoichiometric feed ratio with an oxygen-rich catalyst surface led to the formation of CO2 and H2O as the primary products. For the H-2-pretreated samples, the reaction mechanisms with the catalysts differ. Only Rh/SiO2 is capable of catalyzing the direct oxidation of methane to syngas, while syngas formation over Rh/gamma-Al2O3, Ru/SiO2, and Ru/gamma-Al2O3 can be achieved mainly via a combustion-reforming scheme. The significant difference in the mechanisms for partial oxidation of methane to syngas over the catalysts can be correlated to the differences in the concentration of oxygen species (O2-) on the catalyst surface during the reaction, mainly due to the difference in the nature of the metals and supports. (C) 2002 The Japan Chemical Journal Forum and Wiley Periodicals, Inc.